Physical properties of the NixFe1−xNb2O6 compounds are investigated combining x-ray and neutron powder diffraction with magnetic and calorimetry measurements as well as 57Fe Mössbauer spectroscopy. This system is known to present quasi-one-dimensional magnetism with the magnetic moments arranged along weakly interacting Ising chains. Partial substitution of the magnetic ion tends to suppress the magnetic ordering observed in the end members of the series. When this happens, the low-temperature magnetic specific heat agrees well with what is expected for isolated Ising chains. The lowest temperature powder neutron-diffraction patterns exhibit evidence for the occurrence of short-range order, and analysis of these diffuse neutron-scattering patterns allow us to obtain information on the magnetic correlations. The suppression of magnetism is consistently interpreted as resulting from the magnetic-cation disorder induced by substitution, which enhances the system’s tendency for frustration of geometrical origin.